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High Capacity Garnet-Based All-Solid-State Lithium Batteries: Fabrication and 3D-Microstructure Resolved Modeling

Finsterbusch, Martin and Danner, Timo and Tsai, Chih-Long and Uhlenbruck, Sven and Latz, Arnulf and Guillon, Olivier (2018) High Capacity Garnet-Based All-Solid-State Lithium Batteries: Fabrication and 3D-Microstructure Resolved Modeling. ACS Applied Materials and Interfaces (10), pp. 22329-22339. American Chemical society (ACS). doi: 10.1021/acsami.8b06705. ISSN 1944-8244.

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Official URL: https://pubs.acs.org/doi/10.1021/acsami.8b06705


The development of high-capacity, high-performance all-solidstate batteries requires the specific design and optimization of its components, especially on the positive electrode side. For the first time, we were able to produce a completely inorganic mixed positive electrode consisting only of LiCoO2 and Ta-substituted Li7La3Zr2O12 (LLZ:Ta) without the use of additional sintering aids or conducting additives, which has a high theoretical capacity density of 1 mAh/cm2. A true all-solid-state cell composed of a Li metal negative electrode, a LLZ:Ta garnet electrolyte, and a 25e-6 m thick LLZ:Ta + LiCoO2 mixed positive electrode was manufactured and characterized. The cell shows 81% utilization of theoretical capacity upon discharging at elevated temperatures and rather high discharge rates of 0.1 mA (0.1 C). However, even though the room temperature performance is also among the highest reported so far for similar cells, it still falls far short of the theoretical values. Therefore, a 3D reconstruction of the manufactured mixed positive electrode was used for the first time as input for microstructure-resolved continuum simulations. The simulations are able to reproduce the electrochemical behavior at elevated temperature favorably, however fail completely to predict the performance loss at room temperature. Extensive parameter studies were performed to identify the limiting processes, and as a result, interface phenomena occurring at the cathode active material/solid−electrolyte interface were found to be the most probable cause for the low performance at room temperature. Furthermore, the simulations are used for a sound estimation of the optimization potential that can be realized with this type of cell, which provides important guidelines for future oxide based all-solid-state battery research and fabrication.

Item URL in elib:https://elib.dlr.de/124643/
Document Type:Article
Title:High Capacity Garnet-Based All-Solid-State Lithium Batteries: Fabrication and 3D-Microstructure Resolved Modeling
AuthorsInstitution or Email of AuthorsAuthor's ORCID iD
Finsterbusch, MartinFZJ Jülichhttps://orcid.org/0000-0001-7027-7636
Danner, TimoTimo.Danner (at) dlr.dehttps://orcid.org/0000-0003-2336-6059
Tsai, Chih-LongFZJ JülichUNSPECIFIED
Uhlenbruck, SvenFZJ JülichUNSPECIFIED
Latz, Arnulfarnulf.latz (at) dlr.deUNSPECIFIED
Guillon, OlivierFZJ JülichUNSPECIFIED
Date:11 June 2018
Journal or Publication Title:ACS Applied Materials and Interfaces
Refereed publication:Yes
Open Access:No
Gold Open Access:No
In ISI Web of Science:Yes
DOI :10.1021/acsami.8b06705
Page Range:pp. 22329-22339
Publisher:American Chemical society (ACS)
Keywords:all-solid-state, ceramic, Li battery, microstructure, modeling, continuum
HGF - Research field:Energy
HGF - Program:Storage and Cross-linked Infrastructures
HGF - Program Themes:Electrochemical Energy Storage
DLR - Research area:Energy
DLR - Program:E SP - Energy Storage
DLR - Research theme (Project):E - Electrochemical Prcesses (Batteries) (old)
Location: Stuttgart
Institutes and Institutions:Institute of Engineering Thermodynamics > Computational Electrochemistry
Deposited By: Danner, Timo
Deposited On:20 Dec 2018 14:11
Last Modified:20 Dec 2018 14:11

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